Small-Angle Neutron Scattering: Applications to Multi

Small-Angle Neutron Scattering:
Applications to Multi-Component Systems
Sarah Rogers
ISIS Facility, Rutherford Appleton Laboratory, UK
Neutrons for Science
Neutrons
Where atoms are...
Neutrons
...and what they do
Neutron
Properties
Neutron
Properties
H
Li
C
O
S
X -rays
neutrons
Mn
Zr
Cs
Neutron
Properties
H
Li
C
O
S
X -rays
neutrons
Mn
Zr
Cs
Spallation Neutrons
Accelerator Driven Neutron Source (Spallation)
Accelerator Driven Neutron Source (Spallation)
Target 2
High Energy
Protons
Target 1
excited
nucleus
15-20 neutrons
High energy Proton
The collision of high energy protons with the tungsten nuclei
releases neutrons
Moderators
β„Ž
πœ†πœ† =
π‘šπ‘šπ‘šπ‘š
epi-thermal
Spallation
109
Energy (eV)
106
103
10-5
𝑇𝑇 = 293𝐾𝐾
cold
ultra-cold
100
10-3
10-6
Electronic transitions
Molecular vibrations
Sound modes
Diffusion
Excitations
Polymers and bio-molecules
Lattice spacing
Wavelength (nm)
10-6
hot
thermal
10-4
10-3
πœ†πœ† = 1.798 β„«
10-2
10-1
𝑣𝑣 = 2.20 π‘˜π‘˜π‘˜π‘˜/𝑠𝑠
Structure
100
101
𝐸𝐸 = 25.3 π‘šπ‘šπ‘šπ‘šπ‘šπ‘š
102
L1
L2
Sample
2ΞΈ
Neutron Source
Distance
Neutron Detector
Time-of-flight
𝐸𝐸 =
Time
𝑣𝑣 = 𝐿𝐿1 + 𝐿𝐿2 ⁄𝑑𝑑
1
π‘šπ‘šπ‘£π‘£ 2
2
πœ†πœ† =
β„Ž
π‘šπ‘šπ‘šπ‘š
𝑛𝑛𝑛𝑛 = 2𝑑𝑑 sin πœƒπœƒ
Inelastic Scattering
Scattering: Reciprocal Space
Dynamical Behaviour
Structure: Real Space
Spectroscopy
Molecular Spectroscopy
IRIS
OSIRIS
TOSCA
VESUVIO
MAPS
LET
MARI
MERLIN
HET
Engineering
Large Scale Structures
ENGIN-X
SANS2D
Diffraction
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INTER
POLARIS
CRISP
GEM
SURF
Neutron and Muons
WISH
LOQ
Instruments
PEARL
INES
30
Muons
EMU
MuSR
HIFI
ARGUS
Disordered Materials
SANDALS
NIMROD
Target Station 2 – Phase 2 Instruments
IMAT
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LARMOR
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Neutron & Nanometers
Small-Angle Neutron Scattering (SANS)
Lengthscales probed range from 10s to 100s nm. They are explored in reciprocal space by
detecting the number of scattered neutrons as a function of the scattering vector, Q. Q is
inversely proportional to distance, D, by the approximation:
Detector
Incident beam, wavelength l
q
Sample
Allows the bulk properties of a
material:
β€’ Size
β€’ Polydispersity
β€’ Structure
β€’ Particle Interaction
2πœ‹πœ‹
𝐷𝐷
Units are either Å-1 or nm-1 i.e. the smaller
the value of Q the bigger the object
Scattered beam
Scattering vector, Q
𝑄𝑄 =
Transmitted
beam
Q is also related to wavelength and the
scattering angle by:
𝑄𝑄 =
4πœ‹πœ‹ sin
πœ†πœ†
πœƒπœƒ
2
Q (size) range is varied by altering q or l
β€˜Typical’ Experiment
The 2D SANS patterns obtained are often radially averaged to given an β€˜intensity’, I(Q), vs. Q plot
2D
Radially
average
1D
Modelling
I(Q) contains the information on size, shape and interactions between the scattering centres in the
sample. For monodisperse spheres I(Q) can be defined as:
𝐼𝐼 𝑄𝑄 = ρ𝑝𝑝 βˆ’ πœŒπœŒπ‘šπ‘š 2𝑁𝑁𝑝𝑝𝑉𝑉 𝑝𝑝2𝑃𝑃 𝑄𝑄 𝑆𝑆 𝑄𝑄 + B
Form factor: intra-particle information
- size and shape of particle
Structure factor: inter-particle information.
Depends on the type of interactions in the
system. S(Q) = 1 for dilute dispersions
β€˜Flat background’. Generally
regarded as due to β€˜incoherent’
scattering, often due to
hydrogen
The 1st - Loq
β€’ LOQ was the 1st ISIS SANS instrument and is
positioned on the 50 Hz first target station,
TS-1
β€’ This instrument has demonstrated the
power of SANS at a pulsed source
β€’ Using a fixed sample - main detector
distance of 4 m and neutron wavelengths of
2 to 10 Å at 25 Hz a Q-range of 0.007 – 0.3
Å-1 is accessible
β€’ This Q-range can be extended to 1.4 Å-1 by
employing the wide-angle detector bank
β€’ Extensive sample environments available
β€’ Sample area is the β€˜pit’ which is accessible
via a ladder
β€’ Crane available
For further info contact Steve King: [email protected]
Monit or 3
(only placed in
beam f or
t ransmission
measurement s
Area det ect or
Monit or 2
Frame overlap mirrors
High-angle det ect or
bank
Sample
Monit or 1
Apert ure select or 2
Double-disc chopper
NEUTRONS
25K liquid
hydrogen
moderat or
Apert ure select or 1
Soller supermirror
bender
The present - Sans2d
β€’ Sans2d is the first SANS instrument to be
built on the optimized TS-2
β€’ Operational since 2009
β€’ Detector 1 moves +/- 0.3 m sideways, to 12
m from sample. Detector 2 may be offset to
1.4 m sideways in 3.25 m diam vacuum tank
and rotates to face sample
β€’ Combining the low background and high
flux of Sans2d has allowed weakly
scattering samples to be studied more
efficiently
β€’ Crane available – shared with Zoom
For further info contact Sarah Rogers: [email protected]
100
I(Q) / cm-1
β€’ 2 x 1m2 movable detectors provide a
uniquely wide simultaneous Q range at
good resolution: Q = 0.001 to 3 Å-1, Ξ» = 1.75
to 17 Å
Scattering
from
partially
deuterated polymer shows good
overlap between Sans2d and
Nimrod
Sans2d
NIMROD
10
1
0.1
0.001
0.01
0.1
1
10
Q / Å-1
100
Larmor: Flexible Spin-Echo for Larmor Precession
β€’ Shutter opened on 20th March 2014
β€’ SANS is available now. The spin-echo setup is being
developed with the NWO and TU-Delft over the next
year
β€’ Polarized Beam with Analysis
β€’ Wavelengths 0.5 – 13 Å gives SANS Q range of 0.004 1.6 Å-1
β€’ Length scales of ~20 nm to 20 mm can be studied using
SESANS
β€’ Large block house but detector can move 90° on air pads
β€’ Huber sample stack allows for accurate sample
alignment
β€’ Crane available
For further info contact Rob Dalgliesh: [email protected]
Future 2 - Zoom
β€’ Currently under construction
β€’ Planned open shutter date is November 2016
β€’ SANS will be available from day 1. Polarized and
focusing SANS will be delivered later
β€’ Detector can move to 6 or 9 m from sample
β€’ Vacuum tank can also move 3 m for focusing optics
installation
β€’ Wavelengths 1.75 – 16.5 Å gives Q range of 0.002 - 1 Å-1
β€’ Focusing will allow ultra low Q of 0.0003 Å-1 ~ 2 mm
β€’ Huber sample stack allows for accurate sample
alignment
β€’ Crane available – shared with Sans2d
For further information contact Ann Terry: [email protected]
Polymers in solution for
drug coatings
Solution scattering
Ionic liquid mixtures
Growth of fibrils
Orientation of peptide fibrils
Anomalous relaxation behaviour
in alcohol-water mixtures
Hydrogen loading
Surfactant stabilised
carbon nanotubes
Defects in metals
Interfacial structures of
polymers at various interfaces
Nanoparticles in metal alloys
Interaction of
polymers with DNA
Colloidal crystals
Flux line lattices
Foams
Organic Light Emitting
Diodes (OLEDS)
Templating of nanoparticles with
micelles and microemulsions
SANS
Exchange in nanoemulsions
Interaction of perfume
with micelles
Carbon nanotubes
Movement of drugs through
and into vesicle bilayers
Micellization in CO2
The Sample Environment
Extensive available sample environments allow a broad range of science to be studied via SANS at ISIS.
Sample environment includes:
β€’ Standard ISIS cryostats, furnaces and magnets
β€’ Sample changer with temperature control
(a)
β€’ Linkham stages for advanced temperature control
(b)
I(Q) /cm-1
15
10
β€’ Rheometer and shear cells
time
5
β€’ Pressure cell – 600 bar with stirring. Predominantly used with CO2
β€’ T-jump cell – study non-equilibrium phases
β€’ In-situ DLS and UV-vis
β€’ Grazing Incidence SANS (GISANS)
0
ai + af
Incident beam
ai
Stopped-flow – mixing kinetics
β€’ Well equipped offline labs allow for further characterization
Ø X-ray sets, AFM, BAM, spectrometers
0.04
0.08
0.12
Q /Å-1
Specular peak
af
Yoneda Maximum
Transmitted beam
Ø Study of in-plane structure on the nm lengthscale
β€’
1 mm
0
qy
isotopes
H
Nuclear
Interaction
Changes
D
Li
C
O
S
X -rays
neutrons
Mn
Zr
Cs
Collaboration between University of Bristol and the ISIS SANS
team studying the modification of the physico-chemical
properties of sc-CO2 with surfactants for use in enhanced oil
recovery. Low viscosity of CO2 promotes fingering through
porous media rather than a uniform sweep.
Modifiers commonly used in oily solvents are incompatible with
CO2. Can self assembled custom-made surfactants be used?
Why Neutron and Small Angle Scattering?
surfactant
High penetrating power of neutrons allows a
p-cell with thick windows to be employed
Using D2O allows us to see β€˜nanopools’ of
water in the CO2
Length-scales being probed are ideal for SANS
Na+ or Co2+ or Ni2+n(D2O)
Results
Altering the counterion of the CO2 active surfactant
DHCF4 from Na to Ni or Co causes a viscosity
enhancement of up to 90% compared to pure CO2
Why? Neutrons have the answer! Micelle shape changes
from spherical to wormlike as counterion changes from
Na+ to Co2+ or Ni2+
Langmuir 2010, 26(1), 83-88
Collaboration between Lund University and the ISIS LSS team
studying reversed lipid liquid crystalline nanoparticles as drug
delivery vehicles
These systems are stabilised by low fractions of the surfactant
P80. Location of the P80 within the particle largely control their
function
Why SAS?
Neutrons are non-destructive so samples are
not altered by beam damage
Contrast variation can be used to highlight
specific parts of the system
Length-scales being probed are ideal for SAS
NH3+ NH3+ NH3+ NH3+
OH
OH OH O-
Results
SANS profiles with modelled contributions shown
SANS reveals the core-shell structure of the d-P80
micelles
Hydrogenated tail group
DO
O
O
O
O
w
O
LCNP
CH3
O
O
w + x+ y+ z = 20
DO
OD
P80 micelle
Deuterated head group
diffraction
peak
Results
CV-SANS, CV-NR and SAXS have been used to determine a
detailed picture of the internal structure of the LCNPs,
where the P80 is located within these structures and how
the particles are stabilised
SANS profiles in P80 micelles in H2O (red) and 1:1
H2O:D2O (blue)
Soft Matter 2015, 11, 1140
Work carried out by Infineum studying engine oil
additives which consist of calcium carbonate
nanoparticles – CaCO3 - stabilized by a sulfonate
surfactant. The stability of these particles is crucial for
their correct performance.
The combustion process can produce a considerable
amount of water: how does the presence of water
effect these particles?
CaCO3
Why Neutron and Small Angle Scattering?
H/D Contrast provides direct view of water
Length-scales being probes are ideal for SANS
Ca(OH) layer
Surfactant
Results
CaCO3 particles are spherical with dia. ~5.6nm
Surfactant monolayer is of thickness ~1.8nm
Water layer inserts between the calcium cation at
the surface of the particle and the sufonate anion
1.8nm
5.6nm
Langmuir 2008, 24, 3807 - 3813
Water
0.5nm
Collaboration between University of Sheffield and the
ISIS SANS Team studying transient phases in polymer
crystallisation using a temperature jump (T-jump) cell
designed for SAS beamlines.
Polymer crystallisation is a highly non-equilibrium
process and several different lamellar structures are
possible
Why SANS?
SAS is a powerful technique for studying
lamellar structures
Using selectively deuterated segments, SANS
can provide information on the location and
state of order of such segments
Sample sits here for ambient
conditions
Neutrons
Sample is moved to the heated block
for the SANS measurement
Results
Material C12D25C192H384CHDC11D23 used
Lamellar structures possible are (a) extended chain form,
(b) once-folded chain forn, (c) triple-layer mixed foldedextended (FE) form and (d) alternative models for the
noninteger folded (NIF) form
Results
NIF form has a lifetime of ~ 1minute – time resolution
achievable via SANS
Real-time SANS β€˜snap shots’ reveal structural changes
with time and temperature
Macromolecules 2005, 38, 7201 - 7204
Thanks for listening!
Questions?